臺灣博碩士論文加值系統

目錄
指導教授推薦書
口試委員會審定書
誌謝......iii
摘要......iv
Abstract......v
目錄......vii
圖目錄......xi
表目錄......xv
第一章. 前言......1
第二章. 文獻回顧......3
2.1直接甲酸燃料電池(DFAFC)介紹......3
2.1.1 DFAFC 電池性能探討......7
2.1.2 Pd 觸媒對DFAFC 電池性能的影響......10
2.1.3 Pd 觸媒於陽極下的觸媒毒化與活性衰退......11
2.2石墨烯與氧化石墨烯介紹......14
2.2.1 GO於燃料電池的應用及電池性能探討......16
2.3複合膜材之進料滲透阻隔預測模型......19
2.4觸媒層的探討......22
2.4.1觸媒層內Nafion 接著劑的優量化......23
2.4.2不同觸媒含量的影響......25
2.5氣體擴散層電極製備方式......29
2.6研究動機與目的......32
第三章. 實驗材料與方法......33
3.1 實驗藥品與材料......33
3.2 實驗設備......35
3.3 Graphene oxide(GO)的合成製備......37
3.4 Nafion前處理......40
3.5 Nafion/GO 複合膜材之製備......41
3.5.1 浸漬塗佈製程......41
3.5.2 旋轉塗佈製程......42
3.6儀器分析與操作條件......44
3.7 Nafion膜材性質分析......45
3.7.1 吸水率及膨潤度......45
3.7.2 擴散係數及離子交換容積......46
3.7.3離子導電度測試......47
3.7.4液態甲酸、甲醇與乙醇滲透率實驗......49
3.8觸媒層漿料製備......51
3.9電池性能量測......52
3.10單電池性能測試......54
第四章 結果與討論......55
4.1 GO的分析......55
4.1.1 GO經FESEM的分析結果......55
4.1.2 GO經TEM的分析結果......57
4.1.3 GO經FTIR的分析結果......59
4.1.4 GO經XRD的分析結果......61
4.1.5 GO經Raman的分析結果......63
4.1.6 GO儀器分析結論......65
4.2 Pd與PtRu觸媒對直接甲酸燃料電池影響......66
4.2.1 Pd與PtRu觸媒應用於陽極之電池性能比較......66
4.2.2 Pd觸媒活性衰退的探討......68
4.3市售Nafion 薄膜 (N115、N117、N212) 之性質比較......70
4.3.1 Nafion薄膜之膨潤度與吸水率......70
4.3.2 Nafion薄膜之離子導電度探討......72
4.3.3 Nafion薄膜之甲酸滲透率......74
4.3.4 Nafion薄膜之電池性能探討......76
4.4 自製觸媒層對直接甲酸燃料電池影響......78
4.4.1不同觸媒含量之甲酸燃料電池性能......78
4.4.2 進料濃度對於電池性能之影響......81
4.5 N212/GO 複合膜材分析與電性探討......85
4.5.1 N212/GO 複合膜材之FESEM圖探討......85
4.5.2 N212/GO 複合膜材之XRD探討......89
4.5.3 N212/GO 複合膜材之ATR-FTIR探討......91
4.5.4 N212/GO 複合膜材之Raman探討......93
4.5.5 N212/GO 複合膜材之吸水率及離子交換容積探討......95
4.5.6 N212/GO 複合膜材之離子導電度......98
4.5.7 N212/GO 複合膜材之不同進料滲透率......101
4.5.8 N212/GO 複合膜材之水的擴散係數及進料滲透率探討......106
4.5.9 SC-3.6與SC-0.3之電池性能探討......108
4.5.10 N212/GO 複合膜材之電池性能探討......110
4.5.11 GO於複合膜材中之排列方式......117
第五章.結論......121
參考文獻......124


圖目錄
圖 1. 甲酸燃料電池工作原理示意圖。......6
圖 2. DFAFC於不同甲酸濃度之電池性能。......7
圖 3. sPES薄膜與N115於相同條件下，電池性能之比較。......9
圖 4. 於陽極使用不同Pd金屬比例觸媒對於電池性能的影響。......10
圖 5. 經過一段時間操作後，Pd觸媒活性與電池性能之關係。......13
圖 6. 經過一段時間操作後，Pd觸媒活性與電池性能之I-P Curve。......13
圖 7.石墨烯氧化成氧化石墨烯示意圖。......15
圖 8. 不同掃描速率與產生的電流密度之關係。(a) Pt 奈米顆粒；(b) PtRu奈米顆粒......16
圖 9. GO熱壓於N115上與N115電池性能比較。......18
圖 10. 添加0.5 wt% GO於Recast Nafion中，與N 212電池性能比較。......18
圖 11. Cussler 模型提出之不同排列方式片狀材料。......21
圖 12. 各種比例的Nafion含量在70°C下對於 PEMFC效能的影響。......24
圖 13.於陽極時使用不同觸媒含量對電池性能的影響 (a) 25⁰C ；(b) 70⁰C。......26
圖 14. N117在30°C下(a)不同Pt-Ru觸媒層含量之 I-V Curve ；(b)不同Pt-Ru觸媒層含量之之 I-P Curve。......28
圖 15. 比較CCM與GDE不同方法製備模電極組對於電池性能的影響(a) 循環伏安法；(b)電池性能曲線。......31
圖 16. N212與複合膜材照片圖(a) N212；(b) DC-0.4；(c) DC-2.0；(d) SC-03；(e) SC-3.6。......43
圖 17. 量測導電度的T型cell 圖。......48
圖 18. 液態甲醇滲透實驗裝置圖。......50
圖 19.電池模組與流道板。......53
圖 20. 不同樣品的FESEM分析圖: (a) graphite; (b) GO-1; (c) GO-2; (d) GO-3。......56
圖 21. 不同樣品的TEM分析圖: (a) graphite; (b) GO-1; (c) GO-2; (d) GO-3。......58
圖 22. GO與graphite的FTIR分析圖。......60
圖 23. Graphite 的XRD分析圖。......62
圖 24. GO-1、GO-2與GO-3的XRD分析圖。......62
圖 25. Graphite的Raman分析圖。......64
圖 26. GO-1、GO-2與GO-3的Raman分析圖。......64
圖 27. 自製不同觸媒於陽極下(2 mg cm-2 Pd與PtRu)的GDE電池性能比較。......67
圖 28. 自製Pd觸媒(2 mg cm-2)的GDE電池性能(a) I-P curve； (b) I-V curve。......69
圖 29. Nafion薄膜於不同操作溫度下之離子導電度。......72
圖 30. Nafion薄膜之甲酸滲透率。......75
圖 31. 自製PtRu觸媒(2 mg cm-2)於不同市售Nafion 薄膜 (N117、N115、N212)之電池性能。......77
圖 32. 自製不同觸媒含量(2 mg cm-2 和5 mg cm-2 )的GDE電池性能比較(a) 60ºC； (b) 80ºC。......80
圖 33. 不同甲酸進料濃度及2.0 M甲醇與3.0 M乙醇的電池性能 (a) 60⁰C； (b) 80⁰C I-V圖； (c) 80⁰C I-P圖。......84
圖 34. N212/GO複合膜材之FESEM 表面圖: (a)N212； (b)DC-0.4； (c)DC-2.0； (d)SC-3.6； (e)SC-0.3。......86
圖 35. N212/GO複合膜材之FESEM 側面圖: (a)N212； (b)DC-0.4； (c)DC-2.0； (d)SC-3.6； (e)SC-0.3。 ......88
圖 36. N212與複合膜材之XRD分析圖。......90
圖 37. N212/GO複合膜材與GO之ATR-FTIR分析圖。......92
圖 38. N212/GO複合膜材之Raman分析圖。......94
圖 39. N212/GO複合膜材之離子交換容積與吸水率圖。......97
圖 40. N212/GO複合膜材之擴散係數與5.0 M甲酸滲透率比較圖。......107
圖 41. 80⁰C下1.0 M 甲酸時，SC-3.6與SC-0.3複合膜材之電池性能比較(a) I-V Curve； (b) I-P Curve。 ......109
圖 42. 80⁰C下5.0 M 甲酸 N212/GO複合膜材電池性能比較(a) I-V Curve； (b) I-P Curve。......113
圖 43. 80⁰C下8.0 M甲酸 N212/GO複合膜材電池性能比較(a) I-V Curve； (b) I-P Curve。......114
圖 44. 80⁰C下2.0 M 甲醇 N212/GO複合膜材電池性能比較(a) I-V Curve； (b) I-P Curve。......115
圖 45. 80⁰C下3.0 M 乙醇 N212/GO複合膜材電池性能比較(a) I-V Curve； (b) I-P Curve。......116
圖 46. Nielsen與Cussler模型於5.0 M甲酸進料之相對滲透係數與GO體積分率關係圖。......119
圖 47. N212/GO複合膜材與進料滲透之示意圖。......120

 
表目錄
表 1. 於相同條件下，DFAFC與DMFC之電池性能比較......8
表 2.石墨烯性質......15
表 3.Nafion薄膜於水中之膨潤度與吸水率......71
表 4. Nafion薄膜於不同操作溫度下之離子導電度......73
表 5.Nafion 薄膜於甲酸濃度5.0 M與操作溫度60⁰C下之離子導電度與甲酸滲透率之選擇率......75
表 6. 比較N212/GO複合膜材之吸水率與離子交換容積......97
表 7. 於80⁰C下，N212/GO複合膜材之離子交換容積及離子導電度......100
表 8. N212/GO複合膜材於60⁰C下之滲透率......104
表 9. N212/GO複合膜材於80⁰C下之滲透率......104
表 10. 80⁰C下N212/GO複合膜材之離子導電度與進料滲透率之選擇率......105
表 11. 比較N212/GO複合膜材之水的擴散係數與5.0 M甲酸滲透率......107

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